Descriptor-Driven Computational Design of Bifunctional Double-Atom Hydrogen Evolution and Oxidation Reaction Electrocatalysts for Rechargeable Hydrogen Gas Batteries
Zaichun Liu, Jinlong Yang, Faxing Wang, Yuan Yuan, Taoli Jiang, Zhengxin Zhu, Ke Li, Shuang Liu, Kai Zhang, Weiping Wang, Mingyan Chuai, Jifei Sun, Yuping Wu, Wei Chen
Abstract
Rechargeable hydrogen gas batteries (RHGBs) have been attracting much attention as promising all-climate large-scale energy storage devices, which calls for low-cost and high-activity hydrogen evolution/oxidation reaction (HER/HOR) bifunctional electrocatalysts to replace the costly platinum-based catalysts. Based on density functional theory (DFT) computations, herein we report an effective descriptor-driven design principle to govern the HER/HOR electrocatalytic activity of double-atom catalysts (DACs) for RHGBs. We systematically investigate the d-band center variation of DACs and their correlations with HER/HOR free energies. We construct activity maps with the d-band center of DACs as a descriptor, which demonstrate that high HER/HOR electrocatalytic activity can be achieved with an appropriate d-band center of DACs. This work not only broadens the applicability of d-band center theory to the prediction of bifunctional HER/HOR electrocatalysts but also paves the way to fast screening and design of efficient and low-cost DACs to promote practical applications of RHGBs.